Air electrodes with high catalytic activity are of great importance for rechargeable zinc-air batteries. Herein, a flexible, binder-free composite air electrode for zinc-air batteries is reported, which utilizes a lightweight, conductive, and crosslinked aerogel film of carbon nanotubes (CNTs) functioned as a 3D catalyst-supporting scaffold for bifunctional cobalt (II/III) oxides and as a current collector. The composite electrode shows high catalytic activities for both oxygen reduction reaction and oxygen evolution reaction, resulting from the synergistic effect of nitrogen-doped CNTs and spinel Co3 O4 nanoparticles. Solid-state Zn-air batteries assembled using such free-standing air electrodes (without the need of additional current collectors) are bendable and show low resistances, low charge/discharge overpotentials, and a high cyclic stability.