Porous g-C3N4/TiO2 (MCNT) were successfully synthesized via hydrothermal-calcination method for removal of tetracycline from aqueous solutions. The as-prepared photocatalysts were characterized by XRD, XPS, SEM, TEM, and ESR. The adsorption and photocatalytic experiments show that the optimal g-C3N4 to TiO2 mass ratio is 12:100 (MCNT-12). After adsorption equilibrium, 70 mg of MCNT-12 could remove 88.43% of tetracycline from 70 ml of aqueous solution (10 mg/L) under 90 min xenon lamp irradiation, and only 64.73% of tetracycline is removed by TiO2 under the same conditions. The study shows that this is a synergistic effect of the construction of heterojunction and the adsorption of tetracycline by MCNT through multiple adsorption mechanisms. The quenching experiments and ESR characterization indicate that •O2- is the main active substance in the photocatalytic process. Four cycling photocatalytic tests and reactions in different pH solutions confirmed that the MCNT is a promising photocatalyst for environmental remediation.