The development of novel photocatalysts with high photocatalytic ability is important in the field of photocatalytic degradation and transformation. In this work, we combined ilmenite phase FeTiO3 and TiO2 nanoparticles (P25) through a cross-linking method to produce novel hexagonal FeTiO3/TiO2 composites coated by nanosized TiO2 particles. Their morphology, crystallinity, and light absorption ability were evaluated by scanning electron microscopy (SEM), X-ray diffraction (XRD), and UV-Vis diffuse reflectance spectra (DRS) analyses, respectively. The heterojunction effect between FeTiO3 and TiO2 could promote the spatial separation of photogenerated electrons and holes, gave the FeTiO3/TiO2 composites strong oxidizing ability, and increased absorption of Xe lamp light. When used as photocatalysts toward phenolic compounds and dyes, the 5% FeTiO3/TiO2 composite showed the highest photocatalytic activity. The intermediate product of 4-chlorophenol degradation was also characterized, and the photocatalytic mechanism was proposed. The results indicated that the as-prepared FeTiO3/TiO2 composite materials show promise as a photocatalyst for environmental remediation, which could be applied to water pollution control.