This study compared the effectiveness of relative cerebral blood volume, apparent diffusion coefficient, and spectroscopic imaging in differentiating between primary high-grade gliomas and solitary metastases. A 3.0-T MR unit was used to perform proton MR spectroscopy, diffusion imaging, and conventional MR imaging on 26 patients who had solitary brain tumors (14 high-grade gliomas and 12 metastases). All diagnoses were confirmed by biopsy. Twelve perfusion MR studies (8 high-grade gliomas and 4 metastases) were also performed. The results showed that the choline to creatine ratio and relative cerebral blood volume in the peritumoral regions of high-grade gliomas were significantly higher than they were in the metastases. The apparent diffusion coefficient values in tumoral and peritumoral regions of metastases were significantly higher than they were in the primary gliomas. Although conventional MR imaging characteristics of solitary metastases and primary high-grade gliomas may sometimes be similar, the peritumoral perfusion-weighted and spectroscopic MR imaging enable distinction between the two. Diffusion-weighted imaging techniques were complementary techniques to make a differential diagnosis between the two malignant tumors.