Surface functionalized gold nanorods (GNRs) with three optical signals and the ability to track and observe live cells was investigated. The Cetyltrimethyl Ammonium Bromide (CTAB) was used as the shape-directing agent to develop GNRs with uniform size and aspect ratio. The as-synthesized GNRs can strongly enhance the Raman signal of the attached MGITC on the GNRs. Polyethylene glycol (SH-PEG-COOH) and SH-PEG-FITC were attached with GNRs through ligand exchange with CTAB. They can stabilize the GNRs, reduce the cytotoxicity and provide fluorescence signal. A cell-penetrating peptide was covalently conjugated with SH-PEG-COOH to assist the GNRs to enter living cell. After cultured with the MCF-7 cells, the surfaced functionalized Au nanorods can enter the MCF-7 cells and be tracking with enhanced MGITC Raman signal, FITC fluorescence, and Rayleigh scatter signal.