The low-temperature properties of YbCo2Zn20, which shows a giant specific heat at low temperatures, have been studied by the 59Co-nuclear quadrupole resonance (NQR) technique. The measurement of spin lattice relaxation rate reveals that Yb 4f-electrons unusually persist in a well-localized regime down to at least 0.3K without ordering magnetically. With further lowering temperature, NQR frequency decreases below 0.2K reflecting the lowtemperature Fermi liquid state, even suggesting a crossover to an intermediate valence state in close proximity to the localized-delocalzied transition. We also compare the observed unique properties of YbCo 2Zn20 with those of YbRh2Si2, which shows antiferromagnetic ordering at extremely low temperature. © 2013 The Physical Society of Japan.