The nature of multipolar order and hyperfine-enhanced (HE) 141 Pr nuclear spin dynamics in PrV2Al20 was investigated using the muon spin relaxation technique. No explicit sign of timereversal symmetry breaking was found below the multipolar order temperature TQ ∼ 0.6 K in a zero applied field as anticipated on the basis of the antiferroquadrupolar (AFQ) order picture proposed by Sakai and Nakatsuji [J. Phys. Soc. Jpn. 80, 063701 (2011)]. Further evidence of the nonmagnetic ground state was obtained from the observation of HE 141 Pr nuclear spin fluctuations in the MHz scale. A marked increase in the muon spin-lattice relaxation rate (1/T1,µ) was observed below 1 K with decreasing temperature, which was attributed to the perturbation on the HE 141 Pr nuclear spin dynamics associated with the development of AFQ correlations. The longitudinal field dependence of 1/T1,µ revealed that the enhanced 141 Pr nuclear spin accidentally has an effective gyromagnetic ratio close to that of the muon.