The nuclear magnetic resonance (NMR) spectra of the I=3/2 monovalent ions Na-23, Cl-35, K-39, and Br-79 for NaCl and KBr dissolved into filamentous bacteriophage Pf1 solutions display line splittings and shifts consistent with an interaction between the nuclear spin and the electric field gradient produced by the Pf1 particles. The average electric field gradient and thus the spectral splitting for ions in the void space between magnetically aligned Pf1 particles is modeled using a numerical solution to the Poisson-Boltzmann equation. An NMR titration experiment in a 57 mg/mL Pf1 solution is used to determine the background Na+ ion concentration in solution as 32 mM which compares well with the 31.1 mM negative surface charge on Pf1.