The objective of the present study was to search for medicinal-herb combinations based on Radix Bupleurum chinense DC (“B”), Rhizoma Corydalis yanhusuo WT Wang (“Y”), Caulis Polygonum multiflorum Thunb (“P”), and Flos Albizia julibrissin Durazz (“A”) for antiaging, anxiolytic, and sedative effects. Application of the D-galactose induced accelerated-aging model employing male ICR mice showed that oral administration of some combinations of B, Y, P, and A significantly improved spatial memory in Y-maze test and reduced brain levels of tumor necrosis factor-α and interleukin-6 based on immunoassays and oxidative stress marker malondialdehyde, based on the thiobarbituric acid test, and the loss of whiskers, indicating antiaging and antineurodegeneration effects. In addition, some of the combinatory formulas induced anxiolysis measured using the elevated plus-maze test and/or sedative effects measured using the hole-board test. Over the range of dosages examined, all possible combinations of the four herbs were devoid of any significant side effects in the form of altered locomotor activity, decreased muscle coordination, or anterograde amnesia assessed using the photobeam and rotarod and step-through passive avoidance methods, respectively. The results suggest that various combinations of the B, Y, P, and A herbs could be useful as nonsedative, antiaging and/or antineurodegenerative agents, or anxiolytic agents.