Support properties regulation has been a feasible method for the improvement of noble metal catalytic performance. For Pd-based catalysts, TiO2–CeO2 material has been widely used as an important support. However, due to the considerable discrepancy in the solubility product constant between titanium and cerium hydroxides, it is still challenging to synthesize a uniform TiO2–CeO2 solid solution in the catalysts. Herein, an in situ capture strategy was constructed to fabricate a uniform TiO2–CeO2 solid solution as supports for an enhanced Pd-based catalyst. The obtained Pd/TiO2–CeO2-iC catalyst possessed enriched reactive oxygen species and optimized CO adsorption capability, manifesting a superior CO oxidation activity (T 100 = 70 °C) and stability (over 170 h). We believe this work provides a viable strategy for precise characteristic modulation of composite oxide supports during the fabrication of advanced noble metal-based catalysts.