Trace amounts of three halogens (chlorine, bromine, and iodine) were determined using radiochemical neutron activation analysis (RNAA) for nine sedimentary rocks and three rhyolite samples. To obtain high-quality analytical data, the radiochemical procedure of RNAA was improved by lowering the background in gamma-ray spectrometry and completing the chemical procedure more rapidly than in conventional procedures. A comparison of the RNAA data of Br and I with corresponding inductively coupled plasma mass spectrometry (ICPMS) literature data revealed that the values obtained by ICPMS coupled with pyrohydrolysis preconcentration were systematically lower than the RNAA data for some reference samples, suggesting that the quantitative collection of Br and I cannot always be achieved by the pyrohydrolysis for some solid samples. The RNAA data of three halogens can classify sedimentary rock reference samples into two groups (the samples from inland water and those from seawater), implying the geochemical significance of halogen data.