Ordered mesoporous carbon (OMC) materials have received attention for use as supports in highly efficient catalytic systems because of their excellent properties. We used epoxy compound 2,3-epoxypropyl trimethylammonium chloride (EPTAC) to modify cobalt tetraaminophthalocyanine (CoTAPc) and obtained a novel catalyst (OMC-CoTAPc-EPTAC) based on OMC-bonded CoTAPc-EPTAC that could oxidize Acid Red 1 (AR1) dyes by hydrogen peroxide (H2O2) activation under neutral conditions. OMC enhanced the catalytic performance of OMC-CoTAPc-EPTAC, which resulted in the combined high catalytic activity and high stability. Because of its large surface area and tunable pore texture, OMC has high substrate accessibility, and the modification of the catalyst with EPTAC could promote adsorption of the target substrate into OMC, which achieved the aim of in situ catalytic oxidation with enrichment of the target substrate and improved the catalytic efficiency significantly. Electron paramagnetic resonance spin-trap experiments confirmed that the OMC-CoTAPc-EPTAC/H2O2 system had a nonradical catalytic mechanism, and the high-valent cobalt-oxo intermediates and generated holes were speculated to act as dominant oxidation species for the catalytic degradation of AR1. These results demonstrated a new strategy for the elimination of low-concentration organic pollutants.