The work aims to study effects of silane (GPTMS)-modified coconut shell powder (G-CSP) as an additive on the surface properties of thermoplastic elastomer (TPE) as well as its potential applications. These G-CSP-TPE samples with G-CSP mass fractions of 0, 5%, 10% and 15% were prepared in hot-pressing method. Infrared spectrum tests of GPTMS, CSP and G-CSP were performed with Alpha infrared spectrometer. Surface morphology of G-CSP-TPE samples was observed with MFP-D three-dimensional morphology instrument. Static contact angles of the three different fluids on G-CSP-TPE samples were measured on JC2000CS contact angle instrument. Based on friction pairs consisting of ceramic ball and G-CSP-TPE samples, friction properties of different fluids were investigated with a MFT-5000 friction-wear testing machine at different loads and sliding speeds. The infrared spectrum showed that certain functional groups in GPTMS were successfully grafted into CSP. As the mass fraction of G-CSP increased, both surface roughness and contact angle increased as well. Average friction coefficient of deionized water and sunflower oil were related to sliding speed and load. As sliding speed exceeded 2 mm/s, the average friction coefficient of functioned as a negative correlation with the load. Under the condition of 0.8 N and 4 mm/s, the difference in the average coefficient of friction between deionized water and sunflower oil was the highest. Compared with other G-CSP-TPE samples, 10%G-CSP-TPE sample was more capable of differentiating the average friction coefficient of deionized water and sunflower oil. Based on the 10%G-CSP-TPE sample, average friction coefficient of two types of milk with fat content of 3.6 g/100 mL and 4.4 g/100 mL, was 0.68 and 0.576, respectively. GPTMS-modified CSP can improve surface properties of TPE, and 10%G-CSP-TPE samples are most likely to be used for food taste evaluation and functional food development.