Highly ordered organic semiconductor single-crystal (OSSC) arrays are ideal building blocks for functional organic devices. However, most of the current methods are only applicable to fabricate OSSC arrays of a single component, which significantly hinders the application of OSSC arrays in integrated organic circuits. Here, we present a universal approach, termed three-dimensional (3D) wettability-induced sequential assembly that can programmatically and progressively manipulate the crystallization locations of different organic semiconductors at the same spatial position using a 3D microchannel template, for the fabrication of the two-component OSSC arrays. As an example, we successfully prepared two-component, bilayer structured OSSC arrays consisting of n-type ,'-bis(2-phenylethyl)-perylene-3,4:9,10-tetracarboxylic diimide and p-type 6,13-bis(triisopropylsilylethynyl)pentacene microbelts. The bicomponent OSSCs show ambipolar carrier transport properties with hole and electron mobilities of 0.342 and 0.526 cm V s, respectively. Construction of complementary inverters is further demonstrated based on the two-component OSSCs. The capability of integration of multicomponent OSSC arrays opens up unique opportunities for future high-performance organic complementary circuits.