You're definitely going to want to use, bola, and tranq darts on this one. Too many arrows, will kill it outright(I'm not saying you can't use arrows. You have a high mortality rate if you put more than 3-4 arrows into it), very fragile tame. Bola it about a trikes length away from yourself initially... It's spore, is annoying to deal with.
For an easy tame, wait for the Lymantria to land and then place a tent directly where he/she is at. Its stuck until the tents durability dies out, this gives you enough to build a little house around it for a safe, easy tame.
I tamed the lymantria in early game valguero and it was actually quite easy. All you need to do is use a bola (I used a normal one) and then keep attacking it with a club and it should get knocked out in couple of hits. However, if your trying to tame a higher level one, bring multiple bolas. The saddle is quite cheap so it can be utilised early game.