Metal floating gate electrodes can be formed for a three-dimensional memory device by forming a memory opening having lateral recesses at levels of spacer material layers between insulating layers, depositing a continuous metal layer, and inducing diffusion and agglomeration of the metal into the lateral recesses to form discrete metal portions employing an anneal process. The metallic material can migrate and form the discrete metal portions due to surface tension, which operates to minimize the surface area of the metallic material. Optionally, two or more continuous metal layers can be employed to form discrete metal portions including at least two metals. Optionally, a selective metal deposition process can be performed to deposit additional metal portions including a different metallic material on the discrete metal portions. The metal floating gate electrodes can be formed without employing an etch process. A tunneling dielectric layer and a semiconductor channel can be subsequently formed.