A core property of pervasive computing is smooth data flow with continuous availability across heterogeneous devices. In this context, the multitude of devices, the spontaneous nature of interactions, together with user mobility and frequent disconnections, pose novel challenges to designing secure systems. Furthermore, security related tasks such as setting up secure connections and access control lists, traditionally carried out by trained system administrators, must now be regularly performed by ordinary users. System designers should, therefore, pay special attention to the human factor. This doctoral research aims at defining usable security mechanisms that enable users to securely share information by easily establishing connections between devices and granting access rights to other parties. In this research, we apply usability principles to enable users to bootstrap secure ad-hoc connectivity and manage cross-device, fine-grained access control.