In this study, we employed Co2TiO4 and synthesized ZnO-doped Co2TiO4 nanocomposites, which were utilized as interlayers in silicon-based Schottky photodetectors for optoelectronic characterization. Structural analyses using XRD, SEM, and EDX confirmed successful fabrication. The photodetectors were evaluated across a broad spectral range (351–1600 nm) and under varying light intensities. The incorporation of ZnO nanoparticles significantly enhanced the performance of the Co2TiO4-ZnO/n-Si device compared to its undoped counterpart. Notably, the responsivity (R) improved from 0.35 to 17.39 mA/W at 351 nm and from 1.75 to 23.76 mA/W at 1000 nm. Correspondingly, the specific detectivity increased by nearly an order of magnitude, surpassing 1010 Jones across much of the spectrum. The noise equivalent power (NEP) decreased drastically from 2.16 × 10–10 to 1.03 × 10–11 W·Hz–1/2 at 351 nm and from 4.33 × 10–11 to 7.53 × 10–12 W. Hz–1/2 at 1000 nm, indicating enhanced sensitivity. The external quantum efficiency (EQE) also improved from 0.13 to 6.43% at 351 nm, with sustained enhancement in the UV–vis-NIR regions. Under 20 mW/cm2 illumination, the Co2TiO4-ZnO/n-Si device exhibited a responsivity of 85.99 mA/W compared to 10.23 mA/W for the Co2TiO4/n-Si device, and a detectivity of 4.26 × 1010 Jones, significantly higher than 1.03 × 1010 Jones for the undoped counterpart. These results demonstrate that ZnO doping significantly improves light absorption, carrier transport, and signal-to-noise ratio, making the Co2TiO4-ZnO/n-Si photodetector a promising candidate for high-performance, broadband, self-powered photodetection applications.