The relaxation of an I=3/2 spin system in an anisotropic environment characterized by a finite residual quadrupolar splitting omega(q) is modeled by analytically solving for the density operator from Redfield’s relaxation theory. The resulting equations are cast into the multipole basis in order to describe the tensorial components of the spin density matrix. Included in the relaxation matrix are off-diagonal elements J(1) and J(2), which account for anisotropic systems with omega(q) values less than the width of the resonant line. With the Wigner rotation matrices simulating hard pulses, the response to an arbitrary pulse sequence can be determined. An analytical expression for the response to the double quantum filtered (DQF) pulse sequence (pi/2)-(tau/2)-pi-(tau/2)-theta-delta-theta-AQ for theta=pi/2 is presented, showing explicitly the formation of a second rank tenser owing only to the presence of a finite omega(q). This second rank tenser displays asymptotic behavior when the (reduced) quadrupole splitting is equal to either of the off-diagonal spectral densities J(2) and J(1). Line shape simulations for omega(q) values of less than a linewidth reproduce the general features of some recently reported Na-23 DQF line shapes from biological systems. Distinct relaxation dynamics govern each of the tensorial components of the resonant signal revealing the influence of the experimental variables on the line shape.