"The world is progressing day by day. Within it, the thing that continues to progress the most is electronic technology. And within that, the thing that continues to progress the most is its connection to toys. Now, the number one thing that this is advancing to is creating a 'World of Toys.' "

Several years into the 21st century, technology has been developed to a point where young people can create and customize dolls made to fight using telepathy. At the same time, a young girl named Misaki is sent to live with her aunt in the suburbs of Tokyo, the city where most of the battles take place. On an evening excursion, she finds herself at Tokyo Station without a lift home, and she first witnesses an Angelic Layer battle; Misaki is shocked to see the smaller Angel win against the much larger and clearly stronger one. A lovable lech named Icchan quickly swoops down on her and takes her under his proverbial wing, training her towards becoming a great Angelic Layer combatant.