Mechanisms have been developed for securing computational systems against certain forms of attack. In particular, it has been discovered that, by maintaining and propagating taint status for memory locations in correspondence with information flows of instructions executed by a computing system, it is possible to provide a security response if and when a control transfer (or other restricted use) is attempted based on tainted data. In some embodiments, memory management facilities and related exception handlers can be exploited to facilitate taint status propagation and / or security responses. Taint tracking through registers of a processor (or through other storage for which access is not conveniently mediated using a memory management facility) may be provided using an instrumented execution mode of operation. For example, the instrumented mode may be triggered by an attempt to propagate tainted information to a register. In some embodiments, an instrumented mode of operation may be more generally employed. For example, data received from an untrusted source or via an untrusted path is often transferred into a memory buffer for processing by a particular service, routine, process, thread or other computational unit. Code that implements the computational unit may be selectively executed in an instrumented mode that facilitates taint tracking. In general, instrumented execution modes may be supported using a variety of techniques including a binary translation (or rewriting) mode, just-in-time (JIT) compilation / re-compilation, interpreted mode execution, etc. Using an instrumented execution mode and / or exception handler techniques, modifications to CPU hardware can be avoided if desirable.