CrGeTe3 has recently emerged as a new class of two-dimensional (2D) materials due to its intrinsic long-range ferromagnetic order. However, almost all the reported synthesis methods for CrGeTe3 nanosheets are based on the conventional mechanical exfoliation from single-crystalline CrGeTe3, which is prepared by the complicated self-flux technique. Here we report a solution-processed synthesis of CrGeTe3 nanosheets from a non-van der Waals (vdW) CrGeTe3 template. This structure evolution from non-vdW to vdW is originated from the substitution of Ge atoms on the Cr sites surrounded by fewer Te atoms in the CrGeTe3 lattice due to their smaller steric hindrance and lower energy barrier. These CrGeTe3 nanosheets present regular hexagonal structures with a diameter larger than 1 mu m and excellent stability. They exhibit soft magnetic behavior with a Curie temperature lower than 67.5 K. This non-vdW to vdW synthesis strategy promotes the development of CrGeTe3 in ferromagnetism while providing an effective route to synthesize other 2D materials.