It is an intriguing idea. I'm stepping way out of my already limited knowledge here but it would seem that weight would be the deciding factor. That is either it can lift the payload or it can't. Other hurdles would be easier to address I believe.
As far as the Lancaster actually being considered for this task when I read one of the other posters mention that in the other thread that was the first I had ever heard of it but I did for sure find that interesting.
The weight would not be a factor, considering that the weapons weighed 9,700lb (Little Boy) and 10,300lb (Fat Man).
Lancasters carried the Tallboy (12,000lb) and 12,000lb HC Blockbuster bomb (12,000lb) with just the addition of bulged bomb bays to clear the bombs.
Lancasters also carried the Grand Slam (22,000lb) and Upkeep (9,250lb, not including bomb bay gear to spin it).
Carrying the Grand Slam required extensive modifications, including removing turrets and the bomb bay doors. But it was twice the weight of the A-bombs.
Upkeep was 60" long, the same as the width of Fat Man's tail. It was also 50" in diameter. Overall it was similar in size to Fat Man. But it did hang in the breeze, and required modifications to the bomb bay, including removing the doors.
Little Boy was similar in size to the 4,000lb HC "cookie" - 28" x 120" (30" x 110" for the "cookie").
The Lancaster was considered to carry the initial nuclear bomb, the Thin Man. This was the same diameter as the Tallboy and 12,000lb HC bombs. In terms of length, Thin Man was slightly longer than the 12,000lb HC bomb and about 1m shorter than Tallboy.
To carry this the B-29 would need extensive modifications, the possibility of which was not certain at the start of the project. The Lancaster was brought into consideration if the B-29 could not be modified appropriately to carry the bomb. In the end it was possible and the Thin Man bomb turned out to be a failure, so was never used.
The main deficiencies of the Lancaster were its range, altitude and speed.
The Lancaster could not have dropped the bombs from the base used by the USAAF for the missions. But there were closer options had the need arised, such as Okinawa.
Speed and altitude were more of a problem. The Lancaster I/III's ceiling was in the low 20,000ft range. Not even 25,000ft when unladen, IIRC. But there were the Lancaster VI and Lincoln I which had two stage Merlins, which would have improved the height and speed at which the bomb could be carried.