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A graphene oxide (GO) immobilized with layered double hydroxide (CoAl-LDH/GO) nanohybrid was prepared via a hydrothermal method and characterized by transmission electron microscopy, field emission scan electronic microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy and thermogravimetric analysis (TGA). The TGA results show that the immobilization of CoAl-LDH nanoparticles on GO surface greatly promotes the thermal stability of GO. More importantly, the incorporation of the CoAl-LDH/GO nanohybrid into PF foams leads to not only a great improvement in their mechanical strengths but also a reduction in their brittleness and friability. Specifically, compared to neat phenolic (PF) foam, at only 0.9 phr (parts per hundred of resin by mass) of CoAl-LDH/GO, the compressive and flexural strengths of the modified PF foam increase by 54.8% and 35.2%, respectively, and pulverization ratio decreases by 55.2%. The addition of the CoAl-LDH/GO nanohybrid also results in an increase in the limiting oxygen index and a decrease in the peak heat release of the modified PF foam in cone calorimeter test. Moreover, the thermal stability of the PF foam is enhanced by the addition of the nanohybrid.