I'm using WaterFox because of it's 64-bit native compilation (not 32) because I'm running a 64-bit OS with more than 4GB of RAM. By doing this you avoid the Windows-on-Windows (WOW) emulation/translation layer that bridges all 32-bit applications through your 64-bit operating system (and then to your 64-bit CPU). The other big point of Waterfox is that the regular 32-bit Firefox builds that are released are cross-platform, meaning they work on multiple operating systems such as Linux, Mac OS X, and Windows. The problem with MOST cross-platform software of this nature is that it's almost never optimized for a single operating system or CPU architecture (x86/x86-64, ARM, IBM PPC etc) and since *nix operating systems often use these other CPU architectures the instruction sets can be drastically different with common Intel-compatible instructions for performance being unsupported.
So, what Waterfox actually IS is a native 64-bit compilation (compiled program) of Firefox 9.0's codebase (currently this is the newest final public release) that is optimized for 64-bit operating systems with CPU instruction set extensions for optimization enabled -- stuff like MMX+, SSE & SSE2, eventually SSE3 and SSE4 and soon (hopefully) some AMD64-specific instruction support for 3DNow+ etc.
Waterfox is first and foremost for 64-bit-based operating systems to allow it to have access to extreme amounts of RAM/system memory (much higher memory addressability than 32-bit programs) and for higher performance to be achieved by focusing on the two major (mostly only Intel right now) CPU architectures... Intel and AMD CPU's. By targeting/making use of their hardware instructions for performance specifically (via compiler options and flags turned on that correspond to them), you end up with a noticeably higher performance, faster, more responsive browser.
I haven't tried Pale Moon yet only because the 64-bit compiled offering is based on the now dated Firefox 8.0 codebase where with Waterfox they're already using the 9.0 source code. However, Pale Moon has a 64-bit high performance variant of Mozilla Thunderbird too, which is an e-mail client I use and have used daily for many years.