The luminescence of organic semiconductor materials is the key function for their lighting and display applications. Continuous regulation of emission colors based on one organic molecule system is still a challenge because of their individual emission band. Here we present a novel strategy for modulation of crystal nuclei and growth rates for different crystal phases, which contributes to fine synthesis of the organic polymorph-based alloy microwires that successfully exhibit continuous regulation of emission colors from blue to green. High supersaturation facilitates formation of α-phase microwires with blue emission (CIE [0.17, 0.23]), and low supersaturation is beneficial for self-assembly of β-phase microwires with green emission (CIE [0.29, 0.58]). Impressively, these organic polymorph-based alloy microwires were applied successfully to multicolor display and optical waveguides, which offer potential applications as continuous multicolor emitters for advanced photonics.