Lime mortars and plasters have been used as building materials since the origins of pyrotechnology in the Levant ca. 12,000-14,000 years ago, and currently are experiencing a revival as compatible and sustainable materials in heritage conservation and modern construction. Extensive research has recently explored ways to improve their properties, particularly using Nature as an inspiration. Such a biomimetic approach is enabling the functionalization of lime mortars and plasters via different strategies that are reviewed here and include accelerated setting via enzymatic-like catalyzed carbonation, increased toughness via inter- and intracrystalline additive incorporation, modification of surface wettability and enhanced self-cleaning ability via surface microtexturing and photoactive nanoparticle incorporation, anti-biofouling capacity, increased radiative cooling, or self-healing properties.