Water in the unconfined Kirkwood-Cohansey aquifer system in the New Jersey Coastal Plain contains elevated concentrations (above 3 pCi/L (picocuries per liter)) of the alpha-particle-emitting radionuclide radium-224. Previously, water from the aquifer system had been found to contain radium-226 and radium-228. This observation is of concern because the previously undetected presence of radium-224 may pose an additional, quantifiable health risk that currently is not accounted for by the Maximum Contaminant Level (MCL) of 5 pCi/L for combined radium (the sum of radium-226 plus radium-228 is termed 'combined radium') in drinking water. Water samples were collected from a regional network of 88 wells for determination of concentrations of radium-224, radium-226, and radium-228; gross alpha-particle activity; and concentrations of major ions and selected trace elements. Both gamma and alpha spectroscopic techniques were used to determine concentrations of radium-224, which ranged from <0.5 to 16.8 pCi/L (median 2.1 pCi/L, interquartile range 1.2-3.7 pCi/L). Concentrations of radium-226 and radium-228 in the same samples ranged from <0.5 to 17.4 pCi/L (median 1.7 pCi/L, interquartile range 0.9-2.9 pCi/L) and <0.5 to 12.8 pCi/L (median 1.6 pCi/L, interquartile range, 0.9-2.6 pCi/L), respectively. Concentrations of radium-224 typically were greater than those of the other two radium radionuclides, as evidenced by the highest median, third quartile, and maximum concentrations, as well as the highest concentration among the three radium radioisotopes in 52 (59 percent) of the 88 samples. Concentrations of 5.0 to 5.5 pCi/L of radium-224 result in a gross alpha-particle activity of about 15 pCi/L (the MCL) 36 to 48 hours, respectively, after sample collection when ingrowth of radium-224 progeny radionuclides is considered, even with the unlikely assumption that no other alpha-particle-emitting radionuclide is present in the water. Concentrations of 3.4 to 3.7 pCi/L radium-224 result in a gross alpha-particle activity of 10 pCi/L 36 to 48 hours, respectively, after sample collection when ingrowth of Ra-224 progeny radionuclides is considered. In this latter case, it is possible that the summed alpha-particle activity from radium-226 present at a concentration less than or equal to 5 pCi/L (the MCL for combined radium) and from radium-224 present at a concentration about 3.4 pCi/L or greater may exceed the 15-pCi/L MCL for gross alpha-particle activity. In this study, gross alpha-particle activities were measured within 48 hours after sample collection and were found to exceed the MCL of 15 pCi/L in nearly half (43) of the 88 samples collected. The concentration of radium-224 exceeded that of radium-226 in 55 (62.5 percent) of the 88 samples. Concentrations of radium-224 correlate strongly with those of both radium-226 and radium-228 (Spearman correlation coefficients r=0.74 and 0.91, respectively). Concentrations of radium-224, radium-226, and radium-228 were greatest in the most acidic ground water. Concentrations of radium-224 and combined radium-226 and radium-228 in samples of ground water with pH less than 4.7 exceeded 5 pCi/L in 33 and 67 percent of the samples, respectively. Concentrations of radium-224, radium-226, and radium-228 (measured separately) were greatest in water from the southern part of the aquifer outcrop area. In water from the northern part of the aquifer system outcrop area, radium-224 concentrations were as high as 3.6 pCi/L, and concentrations of combined radium and gross alpha-particle activity in some samples exceeded their respective MCLs. The presence of gross alpha-particle activities greater than 15 pCi/L and combined radium-226 and radium-228 concentrations greater than 5 pCi/L in the southwestern part of the aquifer system outcrop area is common and had been documented before 1997. Results of this study confirm these earlier findings.