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Fe2+-H2O2 Fenton system is widely applied in water treatment nowadays, but the acidification and sludge generation are crucial problems to be solved. Herein, we report that Fe3O4/TiO2/C nanocomposites (FTCNCs) were able to catalyze the decomposition of H2O2 at neutral pH and can be applied in dye decoloration. FTCNCs were prepared by precipitating TiO2 on Fe3O4 cores via the hydrolysis of tetrabutyl titanate followed by the hydrothermal dehydrogenization of glucose to deposit carbon on Fe3O4/TiO2. The decoloration of methylene blue (MB) in the FTCNC-H2O2 Fenton-like system was monitored to reflect the catalytic activity of FTCNC. The radical generation capability was analyzed by electron spin resonance. Our results indicated that FTCNC-H2O2 Fenton-like system was efficient in decolorizing MB, and the radicals led to the near complete oxidation of MB. The FTCNC-H2O2 Fenton-like system could be used in a wide pH range of 4–9. A greater catalyst amount, a higher H2O2 concentration, and a higher temperature accelerated the decoloration kinetics. FTCNCs showed good activity after the regeneration of 8 cycles. The implication to the practical applications of FTCNCs in water treatment is discussed.