Use of dipolar and quadrupolar couplings for quantum information processing (QIP) by nuclear magnetic resonance (NMR) is described. In these cases, instead of the individual spins being qubits, the 2ⁿ energy levels of the spin-system can be treated as an n-qubit system. It is demonstrated that QIP in such systems can be carried out using transition-selective pulses, in CH₃CN, ¹³CH₃CN, ⁷Li (I=3/2) and ¹³³Cs (I=7/2), oriented in liquid crystals yielding 2 and 3 qubit systems. Creation of pseudopure states, implementation of logic gates and arithmetic operations (half-adder and subtractor) have been carried out in these systems using transition-selective pulses.