The last seconds before Itachi died in Sasuke's hand. I thought he would take off Sasuke's eyes in order to get the eternal mangekyou sharingan, but he just hit his little brother's forehead and said,
"Yurusu, Sasuke, kono saigo da," (I'm sorry Sasuke, this is the last time)
Usually Itachi said, "Yurusu, Sasuke, mata kondo da," (I'm sorry Sasuke, maybe next time)
Also when Uchiha Madara told the truth about Itachi. I cried a bit