The synthesis and applications of anisotropic nanostructures have attracted much attention in modern nanotechnology. Recently, biosynthesis has been demonstrated to be a viable green alternative to traditional chemical and physical methods for synthesizing metal nanostructures. Herein, we developed a new, green one-pot synthetic protocol in which silver nanoflowers (Ag NFs) with three-dimensional structures were synthesized by Canarium album foliar broths in the presence of trisodium citrate (TSC) at room temperature. The effects of silver nitrate, TSC, and foliar broths on these synthesis processes were investigated to determine the optimum synthesis conditions. Further exploration of the formation mechanism of Ag NFs showed that both the biomolecules and TSC played very important roles. The improved insight into the specific roles of the bioprotective components and the controlled synthesizing ability are expected to help explain the formation mechanism of this interesting nanostructure that exhibited an excellent performance in surface-enhanced Raman scattering.