Deep Eutectic Solvents (DESs) have emerged as promising candidates to replace conventional organic solvents in various technological applications due to their low vapor pressure, non-flammability, and ease of preparation at low costs. In particular, Type IV DESs, which are composed of metal salts and hydrogen bond donors, are possible replacements for lithium-ion battery electrolytes. In this study, we investigate the molecular dynamics of solvents of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and pyrazole (PYR) at varying LiTFSI:PYR molar ratios (1:2, 1:3, 1:4, 1:5) using Nuclear Magnetic Resonance Dispersion (NMRD) and Pulsed Field Gradient (PFG) Nuclear Magnetic Resonance (NMR). PFG NMR reveals composition-dependent diffusion trends, while NMRD provides molecular-level insights into the longitudinal relaxation rate (R₁ = 1/T₁). Notably, the LiTFSI:PYR (1:2) sample shows distinct behavior across both techniques, exhibiting enhanced relaxation rates and lower self-diffusion for ¹H compared to the other nuclei (¹⁹F and ⁷Li), suggestive of stronger and more efficient Li⁺–pyrazole interactions, as confirmed by the modeling of the relaxation profiles. Our study advances understanding of ion dynamics in azole-based eutectic solvents, supporting their potential use in safer battery electrolytes.