A series of low temperature visible light‐activated black organotitanias were synthesized through a sol‐gel strategy allowing for the in‐situ incorporation of p‐phenylendiamine (PPD) in the framework of anatase nanoparticles. The effect of the synthesis conditions on the crystalline structure and photocatalytic activity of these materials was assessed by a number of characterization techniques, which revealed a small crystalline domain size (4.6‐5.5 nm), the effective incorporation of the PPD inside the nanoparticles, and a significant reduction in the band gap of these materials (from 3.2 eV to 2.7‐2.9 eV). The systematic study of the synthesis parameters allowed us also to significantly reduce the solvent used for the preparation of these black organotitanias (a 20‐fold), as well as the crystallization time, without compromising the structural properties and photocatalytic activity of these materials. The organotitanias with the highest PPD content and high crystallinity result in the best performing materials in the photocatalytic degradation reaction of Rhodamine 6G under both UV and visible light irradiation.