Spinal cord injury (SCI) severity/recovery are influenced by complex pathological mechanisms. We used CEST/NOE MR and TSPO PET imaging to evaluate longitudinal molecular changes associated with neuroinflammation in a lumbar contusion SCI rodent model. The NOE(-1.6 ppm) peak amplitude significantly decreased and the CEST(3.5 ppm) peak amplitude increased in SCI rats, 1-week post-injury. Similarly, we detected significant increase in the uptake of a TSPO-targeting PET radiotracer at the SCI epicenter. The CEST/NOE pools can be linked to neuroinflammatory activity associated with glutamate release. The results indicate that CEST/NOE MRI measurements provide complementary information to TSPO PET measurement in SCI.