The aim of this paper is to define an extension of the controllability and observability forlinear quaternion-valued systems (QVS). Some criteria for controllability and observability are derived, and the minimum norm control and duality theorem are also investigated. Compared with real-valued or complex-valued linear systems, it is shown that the classical Caylay–Hamilton Theorem as well as Popov–Belevitch–Hautus (PBH) type controllability and observability test do not hold for linear QVS. Hence, a modified PBH type necessary condition is studied for the controllability and observability, respectively. Finally, some examples are given to illustrate the effectiveness of the obtained results.