Bimetallic mesoporous Co‐Cr‐TUD‐1 and its counterparts Co‐TUD‐1 and Cr‐TUD‐1 were synthesized by a direct hydrothermal treatment (DHT) method with triethanolamine as a template. The products were characterized by many techniques. Results show that Co and Cr are incorporated into the framework of TUD‐1. The catalytic behaviours of the samples were tested in decomposition of cyclohexyl hydroperoxide (CHHP). Co‐Cr‐TUD‐1 (Si/(Co + Cr) = 25) shows the highest catalytic efficiency with a CHHP conversion of 96.9 % and total selectivity of cyclohexanone and cyclohexanol of 95.9 %, which outperforms Co‐TUD‐1 and Cr‐TUD‐1 and indicates a synergistic effect between Co and Cr in Co‐Cr‐TUD‐1. The catalysts are mainly heterogeneous as shown in various experiments, while the catalytic performances of recovered catalysts declined modestly, indicating non‐negligible amounts of Co and Cr are leached after some cycles.