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Modern energy needs and the pressing issue of environmental sustainability have driven many research groups to focus on energy-generation devices made from novel nanomaterials. We have prepared platinum nanoparticle-decorated silicon nanowire/carbon core&#8722;shell nanomaterials (SiNW/C@Pt). The processing steps are relatively simple, including wet chemical etching to form the silicon nanowires (SiNWs), chemical vapor deposition to form the carbon shell, and drop-casting and thermal treatment to embed platinum nanoparticles (Pt NPs). This nanomaterial was then tested as the counter electrode (CE) in dye-sensitized solar cells (DSSCs). SiNW/C@Pt shows potential as a good electrocatalyst based on material characterization data from Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). Raman spectroscopy shows that the surface reactivity of the SiNW/C is increased by the decoration of Pt NPs. These data also show that the carbon shell included both graphitic (sp<inline-formula> <math display="inline"> <semantics> <msup> <mrow></mrow> <mn>2</mn> </msup> </semantics> </math> </inline-formula> hybridization) and defective (sp<inline-formula> <math display="inline"> <semantics> <msup> <mrow></mrow> <mn>3</mn> </msup> </semantics> </math> </inline-formula> hybridization) phases of carbon. We achieved the minimum charge-transfer resistance of 0.025 <inline-formula> <math display="inline"> <semantics> <mo>Ω</mo> </semantics> </math> </inline-formula>&#183; cm<inline-formula> <math display="inline"> <semantics> <msup> <mrow></mrow> <mn>2</mn> </msup> </semantics> </math> </inline-formula> and the maximum efficiency of 9.46% with a symmetric dummy cell and DSSC device fabricated from the SiNW/C@Pt CEs, respectively.