You should never use structs across compile domains, against memory (hardware registers, picking apart items read from a file or passing data between processors or the same processor different software (between an app and a kernel driver)). You are asking for trouble as the compiler has somewhat free will to choose alignment and then the user on top of that can make it worse by using modifiers.
No there is no reason to assume you can do this safely across platforms, even if you use the same gcc compiler version for example against different targets (different builds of the compiler as well as the target differences).
To reduce your odds of failure start with the largest items first (64 bit then 32 bit the 16 bit then lastly any 8 bit items) Ideally align on 32 minimum perhaps 64 which one would hope arm and x86 do, but that can always change as well as the default can be modified by whomever builds the compiler from sources.
Now if this is a job security thing, sure go ahead, you can do regular maintenance on this code, likely going to need a definition of each structure for each target (so one copy of the source code for the structure definition for ARM and another for x86, or will need this eventually if not immediately). And then every or every few product releases you get to be called in to do work on the code...Nice little maintenance time bombs that go off...
If you want to safely communicate between compile domains or processors the same or different architectures, use an array of some size, a stream of bytes a stream of halfwords or a stream of words. Significantly reduces your risk of failure and maintenance down the road. Do not use structures to pick apart those items that just restores the risk and failure.
The reason why folks seem to think this is okay because of using the same compiler or family against the same target or family (or compilers derived from other compilers choices), as you understand the rules of the language and where the implementation defined areas are you will eventually run across a difference, sometimes it takes decades in your career, sometimes it takes weeks...Its the "works on my machine" problem...
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