The Layer-by-Layer (LbL) method is a well-established method for the assembly of nanomaterials with controlled structure and functionality through the alternate deposition onto a template of two mutual interacting molecules, e.g., polyelectrolytes bearing opposite charge. The current development of this methodology has allowed the fabrication of a broad range of systems by assembling different types of molecules onto substrates with different chemical nature, size, or shape, resulting in numerous applications for LbL systems. In particular, the use of soft colloidal nanosurfaces, including nanogels, vesicles, liposomes, micelles, and emulsion droplets as a template for the assembly of LbL materials has undergone a significant growth in recent years due to their potential impact on the design of platforms for the encapsulation and controlled release of active molecules. This review proposes an analysis of some of the current trends on the fabrication of LbL materials using soft colloidal nanosurfaces, including liposomes, emulsion droplets, or even cells, as templates. Furthermore, some fundamental aspects related to deposition methodologies commonly used for fabricating LbL materials on colloidal templates together with the most fundamental physicochemical aspects involved in the assembly of LbL materials will also be discussed.