Twenty-three soluble (nonparticulate) radioactive agents were screened for their ability to label leukocytes in vitro in the presence or absence of plasma and red cells. The degree of cell binding was compared with that of other agents previously reported. Leukocyte binding of 2% or more of the added radioactivity was obtained with ten of these agents. High labeling yields were obtained only with nonpolar lipid-soluble complexes capable of penetrating lipid cell membranes. Unfortunately, this type of labeling tends to be reduced by plasma protein. Some lipophilic radioactive agents tend to elute from the cells after labeling. Compared with radioactive particles, soluble radiopharmaceuticals offer the advantage of easy centrifugal separation of the cell-bound from the residual activity in the suspension fluid. However, the labeling yield tends to be lower than for radioactive particles, and other cellular elements are labeled in addition to the phagocytic leukocytes. In this survey, the most promising soluble agents were 111In or 99mTc complexes of oxine, 111In-tetraphenylporphyrin, DNA labeled with radioactive iodine, and DNA labeled with 77Br and complexed with adriamycin. The ultimate value of any of these agents must await adequate in vivo testing in experimental animals and clinical trials.