Multimeric compounds that bind to P-Selectin Glycoprotein 1 (PSGL-1) on the surface of T cells or natural killer (NK) cells can be used to induce T cell or NK cell depletion and/or to induce T cell or NK cell apoptosis. The multimeric compounds and methods of the invention can be used to control unwanted T cell-or NK cell-mediated immune responses in conditions such as inflammatory diseases, autoimmune diseases, transplant rejection, and allerg ic diseases.