The nuclear magnetic moment of 9 Li and the quadrupole moments of 8 Li and 9 Li have been measured by use of the β-asymmetry detection of nuclear magnetic resonance on optically polarized beams at ISOLDE/CERN. The radioactive beams were implanted in Si for g-factor measurements and in Zn, LiNbO 3 , and LiTaO 3 crystals for quadrupole moment measurements. The electric-field gradient V zz = 4.26(4) × 10 15 V/cm 2 is deduced for Li in Zn. Using a recently adopted reference value, Q( 7 Li) = −40.0(3) mb, we reevaluated all earlier reported nuclear quadrupole moments of 8 Li and 9 Li. Based on all available previous and present data, the adopted quadrupole moments for these isotopes are Q( 8 Li) = +31.4(2) mb and Q( 9 Li) = −30.6(2) mb. The magnetic moment of 9 Li is deduced as µ( 9 Li) = 3.43678(6)µ N . The values are compared with predictions from shell-model and cluster-model calculations.