Ferroptosis therapy (FT) of the colorectal cancer (CRC) is usually restricted by the relatively slow rate of Fenton reaction due to the limited concentration of intracellular H2O2 and the high-level of endogenous H2S with strong reducibility. To develop an unprecedented strategy for precise targeted CRC theranostics, inspired by the “cyclotron” concept in physics, we propose a new concept of cycloacceleration of ferroptosis and calcicoptosis for the magnetic resonance imaging (MRI)-guided CRC therapy. The developed FGNPs@TA-Fe3/Ca4 nanoparticles have an ideal hydrodynamic diameter of 16.5 ± 2.2 nm and relatively high loading contents of Fe3+/Ca2+ (15.6 ± 3.4 % and 32.1 ± 1.9 %). The powerful T1 imaging ability of FGNPs@TA-Fe3/Ca4 with TME-responsive relaxivities is identified by 7.0 and 3.0 T of MRI scanners. The cycloacceleration of ferroptosis and calcicoptosis induced by FGNPs@TA-Fe3/Ca4 is reinforced by the MTT assay, and the measurements of reactive oxygen species (ROS), lipid peroxide (LPO), glutathione (GSH) peroxidase 4 (GPX4) bioactivity, GSH, H2S and SO2 of CT 26 cells with various treatments with or without ferroptosis or calcicoptosis inhibitors. The in vivo effectiveness and safety of FGNPs@TA-Fe3/Ca4 for MRI-guided CRC therapy based on cycloacceleration of ferroptosis and calcicoptosis are demonstrated on the CT 26 tumor-bearing BALB/c mice.