We present a facile method for fabricating spongelike Au structures by halide-induced aggregation and fusion of gold nanoparticles (AuNPs). Halide ions (F-, Cl-, Br-, and I-) showed distinctly different effects on the synthesized AuNPs, which were characterized by localized surface plasmon resonance (LSPR) and dynamic light scattering measurements. A noticeable red-shift in the LSPR peak was found after Br- and I- ion treatment, which indicates the adsorption of halide atoms or ions on the AuNPs. The surface potential of AuNPs varied by treatment with different types of halides; this finding indicates that different halide ions have different effects on the AuN Ps. Br- and I- ions showed strong affinity toward the AuNPs. The different affinities of halide ions toward the AuNPs play an important role in controlling the formation process of spongelike gold. Citrate ions adsorbed on AuNPs were displaced by halide ions to different extents. Such displacement determined the aggregation and fusion behaviors of the AuNPs and eventually the formation of different spongelike structures.