No.
Memory-aligned means that instructions can only exist on certain addresses. (It also implies a minimum instruction length.) On most RISC architectures, instructions are also a constant size, with the same alignment. For example, a MIPS instruction stream consists of 4-byte instructions aligned to every fourth byte in memory. Memory alignment and constant instruction size ensure that any given instruction stream can only be executed as itself, or part of itself. Note that this is not self-synchronization - if you removed a byte from an instruction stream, you would get a wildly different instruction stream.
(I said MIPS because ARM instruction streams can be THUMB, which permits a different instruction interpretation for the same stream, and thus defeats the security advantages of memory alignment requirements.)
Self-synchronizing means that each subdivided unit (usually byte) of a stream also indicates if it is the start of a new symbol within that stream. For example, UTF-8 is an example of a self-synchronizing byte stream. In UTF-8, encoded codepoints have variable-length representations. However, the upper bits of each byte clearly indicate not only if the byte is the start of a new codepoint, but how many bytes follow to complete the codepoint. This means that a deleted or altered byte will only delete or alter the symbol it's a part of, and not any other part of the stream.
Self-synchronization and alignment requirements address the same problem - ambiguous instruction streams - by different methods. Memory alignment prohibits you from reinterpreting the stream; while self-synchronization makes doing so less valuable.