Wolfram and his team posed as actors who were hired by David and Sam to aid them in orchestrating the villain attack on I-Island in order to steal back their greatest invention - a headset that maximizes the power of its user's Quirk. Whereas David, who was conflicted with the plan, simply wanted to retake the headset so All Might can maintain his status as a hero and keep the world safe with it, as the Symbol of Peace's powers gradually weaken (unknown to him, it all because the hero has passed his Quirk to his apprentice Izuku Midoriya), Sam intended to sell the invention to the villains so he can achieve fame and fortune both he and David denied of. Unknown to either of them however, Wolfram himself is an actual villain who genuinely sought to kidnap David and forced him to mass-produce said invention for his own purposes.
When Wolfram and his team make preparations for the extortion, he was contacted by All For One, who was intrigued by his scheme as it also involved his nemesis All Might. Since they have a common enemy, the Symbol of Peace, Wolfram agreed to have All For One endow him with a Quirk which enabled him to amplify his muscles, and thus counteract his weakness at close range when manipulating metal.
With Sam and David's aid, Wolfram and his team managed to successfully infiltrated I-Island and incapacitated the guards, before proceeded to taking over the island's security system. Afterwards, they made their presence known to inhabitants of I-Island by barging into All Might's reception and assessed them their situation by restraining all pro-heroes and heroes with the island's security system and deter them from resisting. He also coerced David to aid them in opening the island's vault which located at the 200th floor of I-Island's main building, the building the party is hosted at. However, neither he nor his men accounted that Izuku and his friends, Melissa Shield, Tenya Iida, Shoto Todoroki, Momo Yaoyorozu, Ochaco Uraraka, Kyoka Jiro, Minoru Mineta, and Denki Kaminari, who also invited to the island, are still free due to running late for the party.
After the students reach the 80th floor, Wolfram and his team become aware of their plan and attempt to apprehend them as result of Minoru unintentionally triggered the security system. Despite of them managed to have Izuku's friends occupied and restrained by swarms of I-Island Security Bots with 3 of his men failed as rescue of Katsuki Bakugo and Eijiro Kirishima, Izuku and Melissa managed to reach the 200th floor in time to see David and Sam retrieving their confiscated invention that stored in a suitcase and revealed their part in the incident they are in.
After David confessed to both Deku and Melissa his and Sam's part in Wolfram's schemes, Sam double-crossed David by revealing his knowledge that Wolfram and his team are villains all along and attempted to join them for fame and glory they have denied just as Wolfram himself enter the scene. However, Wolfram shoots Sam after getting the suitcase, and David jumps in the way of another bullet in order to save Sam's life. Before Wolfram can kill Melissa, Izuku breaks free in order to fight him. Wolfram uses his Quirk to control metal to hold off Izuku and escapes to the rooftop with the defenseless David in his clutches. He vows to further sink David lower to the path of villainy they are in before putting him out of his misery. Despite his disadvantages over the villains' Quirk, Izuku remained to press on, but failed after Wolfram knocked him off the chopper he and his remaining men used to escape the I-Island, unable to save the rest since Melissa managed to restore the security systems. Fortunately, just as all hope seemed lost, All Might soon appears and snatched David out of the chopper, saving his old friend's life and crashed the chopper into pieces, seemingly killing everyone onboard.
However, Wolfram revealed to have survived the crash: Using Sam and David's invention that bolstered his Quirk, Wolfram builds a gigantic, tentacled behemoth form out of metallic parts of the tower with his human form as a core, all while knocking All Might away from both Melissa and Izuku and imprisoned David inside it. At first, All Might had a hard time against Wolfram's new form until he gained supports from Izuku's friends who arrived at his side which allowed him to went past his limit in order to break through Wolfram' defenses and reached his human form. However, Wolfram soon turned the table by revealing his secondary Quirk, Muscle Augmentation, along with the one who endowed him with it, All For One. Horror-stricken that his old nemesis has an involvement with Wolfram's schemes, All Might is unceremoniously overpowered by Wolfram who proceeded to crush him within his metallic constructs, only for Izuku saved the Symbol of Peace at the very last moments.
Outraged by Izuku's constant interference, Wolfram throws everything he had against the young hero and All Might as the pair rushed for his behemoth form. The battle soon took an epic and devastating proportion with Izuku's friends join the battle by deflecting Wolfram's defenses. Despite his best efforts, Wolfram was ultimately defeated by All Might and Izuku's combined attack, which instantly dismantled his behemoth form, and saved David in process.
Wolfram was last seen among the rubble, with his body deflated and steaming in a similar manner to All Might's True Form. It's unknown what happened to him afterward.