We report results of magnetization and $^{31}$P NMR measurements under high pressure up to 6.4~GPa on RbMoOPO$_4$Cl, which is a frustrated square-lattice antiferromagnet with competing nearest-neighbor and next-nearest-neighbor interactions. Anomalies in the pressure dependences of the NMR shift and the transferred hyperfine coupling constants indicate a structural phase transition at 2.6~GPa, which is likely to break mirror symmetry and triggers significant change of the exchange interactions. In fact, the NMR spectra in magnetically ordered states reveal a change from the columnar antiferromagnetic (CAF) order below 3.3~GPa to the N{e}el antiferromagnetic (NAF) order above 3.9~GPa. The spin lattice relaxation rate $1/T_1$ also indicates a change of dominant magnetic fluctuations from CAF-type to NAF-type with pressure. Although the NMR spectra in the intermediate pressure region between 3.3 and 3.9 GPa show coexistence of the CAF and NAF phases, a certain component of $1/T_1$ shows paramagnetic behavior with persistent spin fluctuations, leaving possibility for a quantum disordered phase. The easy-plane anisotropy of spin fluctuations with unusual nonmonotonic temperature dependence at ambient pressure gets reversed to the Ising anisotropy at high pressures. This unexpected anisotropic behavior for a spin 1/2 system may be ascribed to the strong spin-orbit coupling of Mo-4$d$ electrons.
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