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We report the magnetic and magnetostrictive behaviors of the pseudobinary ferrimagnetic spinel oxide system (1−x)CoFe2O4–xCoAl2O4 [Co(Fe1−xAlx)2O4], with one end-member being the ferrimagnetic CoFe2O4 and the other end-member being CoAl2O4 that is paramagnetic above 9.8 K. The temperature spectra of magnetization and magnetic susceptibility were employed to detect the magnetic transition temperatures and to determine the phase diagram of this system. Composition dependent and temperature dependent magnetostrictive behaviors reveal an exotic phase boundary that separates two ferrimagnetic states: At room temperature and under small magnetic fields (∼500 Oe), Fe-rich compositions exhibit negative magnetostriction while the Al-rich compositions exhibit positive magnetostriction though the values are small (<10 ppm). Moreover, the compositions around this phase boundary at room temperature (x = 0.35, 0.4, 0.45, 0.5) exhibit near-zero magnetostriction and enhanced magnetic susceptibility, which may be promising in the applications for magnetic cores, current sensors, or magnetic shielding materials.