Laser‐induced crystallization was performed to form zero‐dimensional (dot) and one‐dimensional (line) patterns on the surface of Na2Mn0.9Fe0.1P2O7 glass. X‐ray diffraction patterns of crystallized‐glass prepared by conventional heat treatment suggests that the formation of β‐Na2MnxFe1−xP2O7 phase is more likely to form than layered‐ (L‐) Na2MnxFe1−xP2O7, which is the other metastable polymorph. Using the continuous wave (CW) laser‐induced crystallization technique, a demonstration of phase selective crystal patterning was confirmed in Na2Mn0.9Fe0.1P2O7 glass. Depending on the laser power (P), micro‐Raman spectroscopy of dot pattern suggest that three types of structural modifications, that is, softening, crystallization of L‐phase structure polymorph, β‐phase, and a mixture of L‐ and β‐phase, were induced. Meanwhile, the line patterning of Na2Mn0.9Fe0.1P2O7 showed a slow growth rate of 2 µm s−1. At P = 0.73 W, even when scanning was started from the β‐dot, the growth of the β‐line was disturbed by the formation of L‐phase but stable line growth of β‐phase occur at P = 0.76 W. Although the formation rate was also slow, laser irradiation is possible to form metastable polymorph selectively.