EPR spectroscopy can give biologically important information, such as tissue redox status, pO2, pH, and microviscosity, based on variation of EPR spectral characteristics (i.e., intensity, linewidth, hyperfine splitting, and spectral shape of free radical probes. EPR imaging (EPRI) can obtain 1D-3D spatial distribution of such spectral components using several combinations of magnetic field gradients. Overhauser enhanced MRI (OMRI) is a double-resonance technique of electron and nuclear spins. Because the Overhauser enhancement depends on transverse relaxation rate of the electron spin, OMRI can provide pO2 information indirectly, along with a high-resolution MR image. MRI can also indirectly detect paramagnetic behaviors of free radical contrast agents. Imaging techniques and applications relating to paramagnetic species (i.e., EPRI, OMRI, and MRI) have the potential to obtain maximally 5D information (i.e., 3D spatial + 1D spectral + 1D temporal dimensions, theoretically). To obtain suitable dimensionality, several factors, such as the EPR spectral information, spatial resolution, temporal resolution, will have to be taken into account. For this review, the EPRI, OMRI, and MRI applications for the study biological systems were evaluated for researchers to apply the method of choice and the mode of measurements to specific experimental systems.