In this paper, we study the sum secure degrees of freedom (d.o.f.) of two-unicast layered wireless networks. Without any secrecy constraints, the sum d.o.f. of this class of networks was studied by and shown to take only one of three possible values: 1, 3/2 and 2, for all network configurations. We consider the setting where, in addition to being reliably transmitted, each message is required to be kept information-theoretically secure from the unintended receiver. We show that the sum secure d.o.f. can only take one of five possible values: 0, 2/3, 1, 3/2, 2, for all network configurations. To determine the sum secure d.o.f., we divide the class of two-unicast layered networks into several sub-classes, and propose an achievable scheme based on the specific structure of the networks in each sub-class. Our achievable schemes are based on real interference alignment, cooperative jamming, interference neutralization and cooperative jamming neutralization techniques.