To achieve highly efficient adsorbents for radon (Rn), this study prepared bamboo activated carbon (BAC) using bamboo charcoal as the precursor and KOH and NaOH as activators and employed a method of activation by adjusting the pore structure through particle size fractionation. Under the same activation conditions, KOH was consumed less and showed better Rn adsorption performance than NaOH, and the solid milling method saved more activator dosage compared to the liquid immersion method. After carbonizing the bamboo, the highest Rn adsorption coefficients of the bamboo charcoal activated with particle size fractionation (0.43−0.85, 0.25−0.43, 0.18−0.25, and <0.18 mm) were 8.41 ± 0.05, 10.03 ± 0.24, 9.31 ± 0.01, and 8.15 ± 0.21 L/g, respectively under N 2 conditions (at a temperature of 25 °C and humidity of 35%), which were significantly greater than those of bamboo charcoal with overall activation (7.05 ± 0.23 L/g). After optimization, all of the bamboo charcoals with different particle sizes had the highest volume ratio for pores with a diameter of 0.77 nm. BC 0.43−0.85 K1.25 and BC 0.25−0.43 K0.75 maintained 95.74 and 92.36%, respectively, of the original adsorption coefficient after 5 cycles of regeneration under nitrogen. As the bamboo charcoal particle size decreased, the optimal mass ratio of alkali/carbon also decreased. This indicates that particle-size-fractionated activation can reduce the raw material and activator waste. The optimized BAC has a significantly higher Rn adsorption coefficient than the currently used coconut shell activated carbon (4.13 ± 0.51 L/g), making it an efficient and economical adsorbent with excellent application value for radon removal.