var xs from kv in let lst kv Value from item in lst select new List ls

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var xs =
from kv in d
let lst = kv.Value
from item in lst
select new {List = lst, Item = item};
var maxValue = xs.Max(x => x.Item.Val);
var toRemove = xs.First(x => x.Item.Val == maxValue);
toRemove.List.Remove(toRemove.Item);