@Daimler: you're flattering your comparison by ignoring shops/buffets, disabled bogs (all new trains of any kind need at least one) and DVT/second loco (shunting isn't viable on the modern railway, a few off-peak anomalies like the Sleepers aside).
2x67 + Mk4s (all standard, normally 78 seats, but including one SV with 32 seats and one TSOD with 70) would be a better comparison to an actual Voyager - I make that 2.2 seats per metre for a four passenger coach formation (and that's still 132m total length, compared with 116m for a five-car 221).
I'd rather not compare with Mark 4s. While they might seat more than a Mark 2, they're a lot more cramped inside (the density, however, is pretty much identical, at around 3.6spm), and have never been used on XC services. However, I like 87015's DBSO idea. I also think it's unfair to lumber the loco-hauled cross country train with a huge buffet - after all, XC 220s are all buffet free now, with the extra luggage space provided being more than matched by a DBSO's luggage compartment - which is probably more secure too.
However, I can't get round the argument of the disabled toilet - I'll take 8 seats out of a Mark 2 to fit one. So, my loco-hauled set is make up of 67 + X Mk2s + DBSO* (assuming 32 seats), giving these seating densities (I've included those of the Voyagers again for easier reference):
Class 220: 2.3 spm (length 93.3m)
Class 221: 2.4 spm (length 116.1m)
Class 67 + 3 Mk2s + DBSO: 2.2 spm (length 98.8m)
Class 67 + 4 Mk2s + DBSO: 2.4 spm (length 118.4m)
However, for long distance cross country services, 4 1/2 coaches isn't really enough. Let's make up a pair of 220s, for a proper intercity train:
Class 220 x 2: 2.3 spm (length 186.6m)
Class 67 + 7 Mk2s + DBSO: 2.7 spm (length 177.5m)
The longer the train, obviously, the better the seating 'density' of the loco hauled train is - and these trains should be long. In its shortest form, the four-vehicle loco-hauled train doesn't do as well as the four coach Voyager. But, it must be said, four coaches isn't enough for these trains. as the train increases in length (even to just five coaches), we see the loco-hauled stock 'in the lead'. We must also remember that the Mark 2 has just 64 well spaced out seats, all around tables. Newer coaches could increase this - not that I'd want to, as that's one of the Mark 2s' main advantages! I've no doubt that if a new 'class' of stock were commissioned, with higher density seating and a DBSO almost entirely devoted to passenger accomodation, the density would be higher still.
Of course, the Voyager is an extremely poorly designed unit, which is one thing I was trying to highlight! I also feel my second 'table' highlights another issue with these units - the wasted space created by coupling them together, something which you certainly don't find when adding an extra couple of coaches to a loco-hauled train.
*It should be borne in mind that Mk2 DBSOs feature a much larger van area than is the norm across Europe. Elsewhere, this would be almost entirely devoted to passenger accomodation. Still, I'll leave it as it is for the purpose of this comparison.