The concept of ultrathin-film interlamination was demonstrated to be effective for nanostructure control of i-layer of the p-i-n organic solar cells. Crystalline phthalocyanine-amorphous fullerene nanocomposite structure, in which the photogenerated electrons and holes can transport to respective electrodes through spatially separated routes, could be intentionally fabricated. p-i-n cells incorporating interlaminated i-layer showed 1.3% solar energy conversion efficiency.