Light‐harvesting layers in organic bulk‐heterojunction solar cells are commonly fabricated from aromatic solvents which are often toxic or hazardous. To fully omit harmful solvents, (surfactant‐free) nanoparticle dispersions of organic semiconductor blends have been investigated, but only a very limited choice of materials form blend‐nanoparticles. This work is a systematic study of the nanoparticle formation by nanoprecipitation of polymer:fullerene blends. It turns out that miscibility of both components is crucial for the incorporation of the fullerenes into the nanoparticles. This finding demystifies why certain polymer:fullerene combinations seemingly randomly form stable nanoparticle dispersion while others do not. Moreover, the need of miscibility constitutes an important design criterion for processing future semiconductor blends along the nanoparticle route. Some mitigation to the unwanted release of larger amounts of fullerenes can be achieved by using ternary semiconductor blends.This article is protected by copyright. All rights reserved.