The influence of surface modifications on the mechanical properties of epoxy‐hexagonal boron nitride nanoflake (BNNF) nanocomposites is investigated. Homogeneous distributions of boron nitride nanoflakes in a polymer matrix, preserving intrinsic material properties of boron nitride nanoflakes, is the key to successful composite applications. Here, a method is suggested to obtain noncovalently functionalized BNNFs with 1‐pyrenebutyric acid (PBA) molecules and to synthesize epoxy–BNNF nanocomposites with enhanced mechanical properties. The incorporation of noncovalently functionalized BNNFs into epoxy resin yields an elastic modulus of 3.34 GPa, and 71.9 MPa ultimate tensile strength at 0.3 wt%. The toughening enhancement is as high as 107% compared to the value of neat epoxy. The creep strain and the creep compliance of the noncovalently functionalized BNNF nanocomposite is significantly less than the neat epoxy and the nonfunctionalized BNNF nanocomposite. Noncovalent functionalization of BNNFs is effective to increase mechanical properties by strong affinity between the fillers and the matrix. The influence of surface modifications on the mechanical properties of epoxy‐hexagonal boron nitride nanoflake (BNNF) nanocomposites is investigated. The BNNFs chemically surface modified by noncovalent functionalization are prohibited from stacking and aggregation, resulted in homogeneous dispersions in the epoxy matrix with strong interfacial interactions. The incorporation of noncovalently functionalized BNNFs into epoxy resin yields outstanding strength and toughness at low BNNF loadings.