Aramid papers (AP), made of aramid fibers, demonstrate superiority in electrical insulation applications. Unfortunately, the strength and electrical insulating properties of AP remain suboptimal, primarily due to the smooth surface and chemical inertness of aramid fibers. Herein, AP are modified via the nacre-mimetic structure composed of aramid nanofibers (ANF) and carbonylated basalt nanosheets (CBSNs). This is achieved by impregnating AP into an ANF-CBSNs (A-C) suspension containing a 3D ANF framework as the matrix and 2D CBSNs as fillers. The resultant biomimetic composite papers (AP/A-C composite papers) exhibit a layered “brick-and-mortar” structure, demonstrating superior mechanical and electrical insulating properties. Notably, the tensile strength and breakdown strength of AP/A-C5 composite papers reach 39.69 MPa and 22.04 kV mm−1, respectively, representing a 155 % and 85 % increase compared to those of the control AP. These impressive properties are accompanied with excellent volume resistivity, exceptional dielectric properties, impressive folding endurance, outstanding heat insulation, and remarkable flame retardance. The nacre-inspired strategy offers an effective approach for producing highly promising electrical insulating papers for advanced electrical equipment.