Shinji begins attending his new school in Tokyo-3, and has a difficult time dealing with the fame of being an Evangelion pilot. Touji Suzuhara, who's little sister was injured in Shinji's fight against the Angel, is angry at Shinji. A new Angel appears, and Shinji must once again pilot EVA-01 to defeat it.

Misato is upset with Shinji for ignoring her orders in the last Angel battle, and he is so overcome by the stress of being an EVA pilot that he runs away. After wandering around Tokyo-3 for several days, Shinji is faced with the choice of quitting or staying in his new home.

EVA-00 is finally repaired, and Shinji tries to get to know its enigmatic pilot, Rei Ayanami, better. However, he is confounded because she is extremely insular, has no friends at all, and the entire record of her past has been erased. In the midst of this, a very powerful Angel, the floating monolith Ramiel, attacks Tokyo-3.

Continuing from the previous episode, the Angel Ramiel is drilling down into the GeoFront to attack NERV HQ directly. After Shinji barely survived a direct confrontation with it, Misato devises a plan to have EVA-00 and EVA-01 defeat the Angel by sniping it from a distance using a positronic rifle which requires the total electric output of Japan to power up.

Misato brings Shinji, along with Touji and Kensuke, to a massive UN naval convoy transporting Evangelion Unit-02 and its fiery German pilot, Asuka Langley Souryuu, to Japan. Escorting Asuka is Misato's old boyfriend, Ryouji Kaji. After some awkward introductions and reunions, the fleet is attacked by a massive aquatic Angel. Asuka powers up Eva-02, and decides that she will defeat the Angel by playing "hopscotch"...

Asuka joins Shinji’s class at school, and moves in with Misato and him in their apartment. As Asuka adjusts to Japan (or rather, everyone else adapts to her...), a new Angel attacks which is capable of splitting itself into two identical copies. EVA-01 and EVA-02 are defeated, and NERV is publicly humiliated. With the Angel in a week-long regeneration period after an N² Mine attack by the JSSDF, Asuka and Shinji must learn to "synchronize" with each others movements combat, in order to defeat it once and for all.

The EVA pilots are disappointed to find out that they are not allowed to go on their class trip to Okinawa, because they have to stay at Tokyo-3 to stay on-call in case of an Angel attack. Meanwhile, a new Angel is discovered in a chrysalis-like developmental stage deep within the magma of the volcano Mount Asama.

Misato has been promoted to Major, but the celebration does not last long. A monstrous Angel appears in Earth orbit right when Gendo and Fuyutsuki are away, leaving her and the children to deal with a colossal kamikaze threatening to drop itself right on top of Tokyo-3.

In the first half of the episode, a clip show is presented to the Human Instrumentality Committee of Seele, reviewing the attacks of all Angels up to this point. The second part includes a poem in which Rei contemplates her own existence, and a cross-compatibility test between Rei's and Shinji's EVAs.

It seems like it's an important day for nearly everyone at NERV. Misato and Ritsuko are going to a wedding; Shinji and Gendo are visiting Yui's grave; Asuka has a date. However, important things will spring from these seemingly mundane events.

A NERV branch in Nevada is obliterated in a catastrophic accident, and NERV headquarters prepares to station a new Evangelion in Japan. The Fourth Child is selected, unbeknownst to Shinji.

Evangelion Unit-03 arrives from the United States. However, its activation experiment brings out NERV's worst nightmare when it turns out to have been infected by the Thirteenth Angel. The other EVAs are dispatched to battle the Angel-infected abomination... even at the risk of killing its helpless pilot.

Enraged over Touji's near-death at the hands of his own EVA, Shinji refuses to pilot an Evangelion again and prepares to leave Tokyo-3 for good. He is forced to reconsider that decision when an immensely destructive new Angel attacks just as he is about to leave...

Instrumentality continues. The focus is primarily on Shinji now, as he learns to accept the individual’s ability to shape their world, and how the self cannot exist without others to define it.