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I would argue that FIPs and most of the TTO pitcher systems are designed to be very good "in the center", but tend to break down severely as you run into outlier (low example) combinations.
Remember that the formulas for these stats are based on actual ERAs (over time) for a large population of pitchers, and because of that, they can successfully factor out defense.  And they work -- IN THE CENTER.
At the fringes, these stats almost never match ERAs ... either individually or as a group, (from my observations).
How many comps does Morrow really have?  How many 10-K SPs have there been in all of history?  How many walked 4.5 to 5 guys a game?  If your comps consist of Hideo Nomo and early career Nolan Ryan ... and not much else, what is that actually supposed to say?
But, ultimately, I think the real picture is that when your stats are SO extreme, you game results do not even out nicely.  Morrow doesn't actually throw 10 Ks and walk 5 games a game.  He fans 14 with 3 walks one game and walks 7 and fans 6 the next.  His ERA totals are high because his hits and walks "naturally" bunch up (mostly depending on his control on any given day).  And ERA is driven up (over FIPs) because run scoring events get bunched instead of spread out.  For somebody like ...Vargas, too much bunching is probably more luck.  For a guy like Morrow, it's a reality of the complete (erratic) package that he is.