Much more to it actually...
Barrel and crown are important, but so are:
a. alignment of each chamber to the barrel, left/right, up/down.
b. is each chamber aligned the same?
c. does it shoot all six chambers to the same group or are one or more consistently shooting their rounds out of the group?
d. throat size needs to be consistent chamber to chamber, and between groove diameter (barrel .357"/throat .357") or up to .001" over groove diameter.
e. cylinder lockup should not be sloppy but neither should it be tight. There should be a slight bit of rotational movement. This allows the bullet as it leaves the throat to align with the barrel's forcing cone.
f. The forcing cone should be cut and finished properly. A lot of different opinions on this but many agree a 11 degree cut is correct with the tool marks polished out. Deep enough to guarantee a smooth transition into the barrel but not larger than it needs to be.
g. The barrel should not be "choked" or tight where it screws into the frame (just in front of the forcing cone). If tight, it can be lapped out.
h. Last, and very important, grips. Not only to give you the right relationship to the trigger, but to put the gun at the proper angle for accurate shooting. I used Nill Hemphill PPC grips throughout my career to good effect.
In my Bullseye career shooting a revolver I went through MANY revolvers before I settled on having Hamilton Bowen build me a custom gun. He addressed each of the issues above (and more) and the gun is incredibly accurate - 5/8" groups at 25 yards and 1.5" at 50 with Winchester "White Box" 148 grain WC ammunition.
With Nills when competing
With Culina target grips now
Hope this helps.
Keith