Hardest for me to catch was: Groudon, nearly 40 Ultra Balls, also had him asleep and false swiped down to nothing, but it took me over 50 minutes to catch him because he kept using Rest and healing up, and Delcatty was getting destroyed by Lava Plume every time
Easiest Catch: Palkia, 3 Ultra Balls lol
Reshiram was pretty quick for me also, same with the Swords of Justice, Uxie and Mesprit were quick, Azelf was just kicking my butt
raikou was a pain in the butt because he kept paralyzing my team, the other 2 Legendary Beasts were fast, Tornadus was pretty quick and Ho-Oh was not bad to catch
my secret was using false swipe then either stun spore from Venusaur, Sing from Delcatty or Raikou's Thunder Wave, either way it was bring their health down and then some kind of sleep or stun