Background: Intracranial space-occupying lesions (ICSOL) encompass a variety of pathologies, ranging from primary brain neoplasms and metastatic tumors to infections. Although Magnetic Resonance Imaging (MRI) is fundamental for initial localization and characterization, certain lesions display overlapping morphologic features. In these scenarios, Magnetic Resonance Spectroscopy (MRS) provides additional metabolic information, aiding in the distinction between benign and malignant processes. Methods: This prospective investigation took place at a tertiary care center in India. Thirty-nine individuals with ICSOL on conventional MRI were considered, and among them, 30 underwent MRS using a 3T MRI system equipped with spectroscopic functionality. Single-voxel or multi-voxel techniques were employed to determine metabolite ratios—such as Cho/Cr, NAA/Cr, and Cho/NAA—and to detect minor metabolites including lactate, lipids, alanine, and amino acids. Standard thresholds were used to characterize lesions. Final diagnoses were confirmed by histopathology or microbiological analysis. Results: Of 39 patients, 30 produced analyzable spectroscopic data. Headaches (71%) and seizures (46%) were the most common symptoms. Gliomas constituted the largest subset (56%), followed by metastatic lesions (10%); 23% were infection-related. High-grade gliomas demonstrated markedly elevated Cho/Cr ratios as well as lactate–lipid peaks. Meningiomas were associated with alanine peaks, while abscesses often showed amino-acid resonances. The combined accuracy of MRI+MRS (83.3%) surpassed that of MRI alone (71%). Conclusion: MRS provides valuable biochemical insights that complement standard MRI for diagnosing ICSOL. Characteristic spectral patterns, particularly changes in choline and N-acetyl aspartate along with specific minor metabolites, facilitate differentiation of high-grade and low-grade tumors and help distinguish infections from necrotic tumors. This integrated approach is beneficial for guiding focused biopsies, optimizing treatment decisions, and assessing post-therapy alterations.