Biocompatible nanoparticles (NPs) responding to the light, thermal, or magnetic excitation are attracting more attention for diagnosis and therapy of cancer. Design of an effective multifunctional complex based on those NPs is a key issue to be addressed, for example, integration of anti-tumor agents with nanoprobes has been considered as one of the successful strategies for combined cancer diagnosis and therapy. In this paper, we develop paclitaxel (PTX)-loaded PEGylation KMnF3 NP, with the size ranged from 18 to 23 nm, as MRI contrast agents for cancer imaging and drug delivery for chemotherapy. Preliminary cell tests demonstrated that PTX@PEG-KMnF3 NP is highly biocompatible. The NP has high loading capacity of PTX (0.7 mg PTX/mg Mn ions), enhanced solubility of PTX (0.16 mg PTX/ml vs 0.02 mg PTX/ml), and high releasing ratio (90 %) in the weak acid solution. As it was applied for in vivo imaging and therapy, the NP enhanced contrast of tumor’s MR images and PTX’s anti-tumor effect profoundly. The signal noise ratio of the cancer image increased 170 % as comparison to pre-injection with the injection dose of 1.15 mg Mn/kg. The drug delivery’s efficacy was also substantially improved, as the tumor growth inhibition effects reached 50 %, meanwhile only 30 % for pristine PTX. Our studies suggest that PTX-loaded KMnF3 NP might be useful as MR image-guided drug delivery for tumor treatment.