Environmentally friendly, flame-retardant, and relatively low-density (0.25-0.31 g cm −3 ) silicone foams (SiFs) were successfully obtained through dehydrogenation at room temperature (RT = 25.0 C). Moreover, a flame-retardant system for SiFs was obtained through a synergistic combination of platinum (Pt) compounds, superfine aluminum hydroxide (ATH), and ultrafine calcium carbonate (CC). The smoke suppression, flame retardance, mechanical properties, and thermal stability of SiFs with Pt compounds, ATH, and CC were tested using the limited oxygen index (LOI), UL-94 test, smoke density test, cone calorimeter, and thermogravimetry-Fourier transform infrared spectroscopy. With only 0.6 wt % Pt compounds, the pure SiF achieved the UL-94-V1 rating (3 mm thick), had an LOI value of 29.6%, and the maximum smoke density (MSD) was 6.5%. After adding ATH and CC, SiF composites could achieve the UL-94-V0 rating (3 mm thick), the LOI increase to 35.2%, and MSD decrease by 45%. Furthermore, the SiF with 0.6 wt % Pt compounds, 15.0 wt % ATH, and 15.0 wt % CC exhibited the optimal comprehensive properties for smoke suppression, flame retardance, mechanical performance, and thermal stability.