Assuming that you use the original 64x32 pixels matrices, this would be an array of 2x2 panels, which - and this is the significant part - would also require an vertical alignment (besides the horizontal one).
Back in the days I have also played around with many combinations or display chaining, and I thought I would also have aligned the matrices vertically - but obviosly my memory must be wrong…
I checked back the Picographics specification and it still reads only one possible combination of chaining displays together vertically and this is 128x128 using two vertically arranged 128x64 displays. Any other vertical arrangement should not be supported as of now.
So far nothing new for you.
So, basically the resolution which you want is, what’s supported already: 128x64
And even two of those can be vertically chained together.
Thus, the conclusion is: It’s just a logical thing rather than a physical thing, as twice of the frame buffer can be addressed already and handled by Interstate75, it should be no big deal for @Pimoroni to update the PicoGraphics library and make us all happy…
So, rather than doing some mapper coding myself to mitigate, I propose to file a feature request on the github site to have this new thing brought to life for all of us…
…because I also would like to see some new fancy resolutions, such as four 64x32 displays arranged vertically for some fancy retro gaming machines or so…
…it’s no impossible ask, as they are aware of already and open to future improvements, which they also state on the spefcification site…

As @Gadgetoid from Pimoroni is the maintainer of the library and I know he is versatile guy, he would probably be able (willing) to easily incorporate some new fancy resolution schemes for us with ease; to realize our lovely projects.
Maybe we should collect some of our resolution wishes here and let him change this at once in May or so…
I vote for any possible combination of horizontal as well as vertical alignments of up to four displays with resolutions of 64x32 and 128x64 pixels.
This would resolve into the following:
====================[ 64x32 ]====================
1:1 = 64x32
horizontally:
2:1 = 128x32
3:1 = 192x32
4:1 = 256x32
vertically:
1:2 = 64x64
1:3 = 64x96
1:4 = 64x128
====================[ 128x64 ]====================
1:1 = 128x64
horizontally:
2:1 = 256x64
3:1 = 384x64
4:1 = 512x64
vertically:
1:2 = 128x128
1:3 = 128x192
1:4 = 128x256