β-NMR spectra have been observed for 33Cl, 23Al and 23Ne. As a result, the magnetic moment of 33Cl was determined as μ(33Cl) = 0.7549(3) μN. Combined with the known magnetic moment of 33S and the ft-value of the 33Cl β decay, the orbital angular momenta and the intrinsic spins for proton and neutron groups, are deduced separately as 〈l p〉 = 1.3, 〈n〉 = 0.3, 〈S p〉 = -0.12 and 〈Sn〉 = -0.02. The magnetic moment of 23Al, and that of 23Ne were determined as μ(23Al) = 3.89(22) μN and μ(23Ne) = 1.0817(9) μN, respectively. As a result, the orbital angular momentum 〈lz〉 and the intrinsic spin 〈S z〉 were deduced to be 2.09(29) and 0.41(29), respectively. Combined with the ft-value of the β transition from the ground state of 23Al to the excited state of 23Mg, proton and neutron contributions are separated. The obtained expectation values 〈l p〉, 〈ln〉, 〈Sp〉 and 〈Sn〉 are compared with the shell model predictions.