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A versatile and simple method is presented for the rapid fabrication of close‐packed colloidal 2D crystals with large domain sizes by floating and redeposition of colloidal monolayers at the air/water interface. A detailed analysis of the particle surface transformation and packing during the individual steps of the monolayer fabrication process has been conducted. It was found that the quality of the monolayer depends on parameters like colloidal particle distribution on the initial substrate, subphase pH, and addition of surfactants. The floating monolayers could be transferred and stacked onto many substrate types, regardless of surface polarity, roughness, or curvature.