The effect of activated carbon particle diameter (i.e. US sieve No. 8×10 (dp ≈ 2.19 mm), 18×20 (dp ≈ 0.92 mm), 50×60 (dp ≈ 0.27 mm) and 170×200 (dp ≈ 0.081 mm)) on caffeine adsorption is investigated. BET surface area was increased with decreasing particle diameter (dp), and caffeine adsorption rates increased with decreasing dp. Moreover, pseudo-second order model is predicted the experimental data more accurately than pseudo-first order model, and the fastest rate constant (k2) was 1.7 g mg-1 min-1 when dp was 0.081 mm. Surface diffusion coefficient (Ds) was decreased with decreasing dp based on the minimum sum of square error (SSE). Practically, certain ranges of Ds are acceptable with high reliability (R2) and it is determined that the effect of dp on Ds is unclear. The effect of pH on caffeine adsorption indicated the dependency of m/L ratio (mass liquid ratio) and pHPZC. The pHPZC (i.e. 7.9 ± 0.2) was not affected by dp. The higher caffeine adsorption at pH 4 and pH 7 than at pH 10 is due to pHPZC, not pka of caffeine.