To describe the interfacial dynamics between two phases using the phase-field method, the interfacial region needs to be close enough to a sharp interface so as to reproduce the correct physics. Due to the high gradients of the solution within the interfacial region and consequent high computational cost, the use of the phase-field method has been limited to the small-scale problems whose characteristic length is similar to the interfacial thickness. By using finer mesh at the interface and coarser mesh in the rest of computational domain, the phase-field methods can handle larger scale of problems with realistic interface thicknesses. In this work, a C1 continuous h-adaptive mesh refinement technique with the least-squares spectral element method is presented. It is applied to the Navier–Stokes-Cahn–Hilliard (NSCH) system and the isothermal Navier–Stokes–Korteweg (NSK) system. Hermite polynomials are used to give global differentiability in the approximated solution, and a space–time coupled formulation and the element-by-element technique are implemented. Two refinement strategies based on the solution gradient and the local error estimators are suggested, and they are compared in two numerical examples.