In this paper, we mainly focused the approximate controllability results for a class of non-densely defined fractional neutral differential control systems. First, we establish a set of sufficient conditions for the approximate controllability for a class of fractional differential inclusions with infinite delay where the linear part is non-densely defined and satisfies the Hille-Yosida condition. The main techniques rely on Bohnenblust- Karlin's fixed point theorem, operator semigroups and fractional calculus. Further, we extend the result to study the approximate controllability concept with nonlocal conditions. Finally, an example is also given for the illustration of the obtained theoretical results.