Strong interplay of spin and charge/orbital degrees of freedom is the fundamental characteristic of the iron-based superconductors (FeSCs), which leads to the emergence of a nematic state as a rule in the vicinity of the antiferromagnetic state. Despite intense debate for many years, however, whether nematicity is driven by spin or orbital fluctuations remains unsettled. Here, by use of transport, magnetization, and 75As nuclear magnetic resonance (NMR) measurements, we show a striking transformation of the relationship between nematicity and spin fluctuations (SFs) in Na1-xLi x FeAs; For x ≤ 0.02, the nematic transition promotes SFs. In contrast, for x ≥ 0.03, the system undergoes a non-magnetic phase transition at a temperature T0 into a distinct nematic state that suppresses SFs. Such a drastic change of the spin fluctuation spectrum associated with nematicity by small doping is highly unusual, and provides insights into the origin and nature of nematicity in FeSCs.