If it's a question of performance, with enough cores and shared memory that's accessible for atomic operations, I'd think talking to a userland filesystem would just* be a matter of pushing requests onto a lock-free request queue in shared memory from your application process and reading the responses from a lock-free response queue. Of course each application needs its own shared-memory area for talking to the filesystem to get fault isolation.
Even if it's a matter of IPC message-passing cost on a single core, I think L4 has shown how to make that cheap enough that we should regard putting the filesystem in the kernel as a dubious optimization, and at that one that's second-best to granting the application mappings on an NVDIMM or something.
Perhaps this is stating the obvious, but I don't think you can get much fault isolation with a pure library filesystem; if all the processes participating in the filesystem are faulty then there's no way to protect the filesystem from fatal corruption from faults. You might be able to reduce the presumed-correct filesystem core process to something like a simplified Kafka: a process that grants other processes read-only access to an append-only log and accepts properly delimited and identified blocks of data from them to append to it.
If we're interested in efficiency and simplicity of mechanism, though, a library filesystem is likely faster and might be simpler than a conventional monolithic filesystem server, particularly a single-threaded one, because you can rely on blocking I/O. And the library might be able to wrap updates to the persistent store in lock-free transactions to reduce the frequency of filesystem corruption.
The Xerox Alto famously used a single-tasking library filesystem similar to MS-DOS, but each sector was sufficiently self-describing that filesystem corruption was usually minor and easy to recover from. The filesystem directory could be reconstructed from the data blocks when required. Neither the Alto nor MS-DOS had to worry about locking, though!
KeyKOS, as you know, took a lot of the ideas from the CAP machine and similar capability machines (and languages like Smalltalk), and implemented them on IBM 370 hardware using its regular MMU, with L4-like lightweight IPCs through the kernel for capability invocations. It went to the opposite extreme from having a library filesystem: each directory and each file was a "domain" of its own, which is to say a single-threaded process. Persistence was handled by a systemwide copy-on-write snapshot of the whole system state, plus a journal-sync call their database used to provide durable transactions. EUMEL and L3 took similar approaches; L4 instead takes persistence and even virtual memory out of the kernel.
I wrote some somewhat sketchy notes on how Flash performance suggests rearchitecting things the other day at https://news.ycombinator.com/item?id=31902551; I know you have a very substantial amount of experience with this as a result of Varnish and your involvement with Fastly. What do you think?
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* "Just" may be a loaded term here.