Feasibility of multiwavelength Raman spectroscopy was studied as a potential in-line monitoring technique for grain size distribution in channel poly-Si used in three dimensional stacked NAND (3D NAND) Flash memory devices. Various channel poly-Si materials in 3D-NAND Flash memory devices, converted from chemical vapor deposition (CVD) grown a-Si, were characterized using non-contact, multiwavelength Raman spectroscopy and high resolution cross-sectional transmission electron microscopy (HRXTEM). The Raman characterization results were compared with HRXTEM images. The correlation between the grain size distribution characterized by multiwavelength Raman spectroscopy and “on current” (ION) of 3D NAND Flash memory devices was investigated. Good correlation between these techniques was seen. Multiwavelength Raman spectroscopy is very promising as a non-destructive in-line monitoring technique for grain size distribution in channel poly-Si used in 3D NAND Flash memory devices.