Sandwich-structured nanocomposites have the potential to improve the mechanical and electrical properties of materials simultaneously. Nanofibrillated cellulose (NFC) modified paper sheet (denominated as N) and softwood paper sheet (denominated as P) are used to prepare insulating paper. Different kinds of insulating paper with the structures of PPP, NNN, NPN and PNP are prepared. Tensile strength, DC conductivity, dielectric response, space charge and breakdown strength are measured. The activation energies of prepared materials are calculated through DC conductivity at 30, 50, 70, and 90 °C. The mechanism for sandwich structure regulating the mechanical and breakdown properties of insulating paper is discussed. Oil impregnated N/P/N paper has a remarkable improvement on tensile strength, conductivity, and DC breakdown strength, which provides a promising scheme to obtain the insulating paper with outstanding tensile and breakdown strength.